Issue 3, 2021

Particle shape tunes fragility in hard polyhedron glass-formers

Abstract

We demonstrate that fragility, a technologically relevant characteristic of glass formation, depends on particle shape for glass-formers comprised of hard polyhedral particles. We find that hard polyhedron glass-formers become stronger (less fragile) as particle shape becomes increasingly tetrahedral. We correlate fragility with local structure, and show that stronger systems display a stronger preference for a pairwise face-to-face motif that frustrates global periodic ordering and gives rise in most systems studied to bond angle distributions that are peaked around the ideal tetrahedral bond angle. We demonstrate through mean-field-like simulations of explicit particle pairs and surrounding baths of “ghost” particles that the prevalence of this pairwise configuration can be explained via free volume exchange and emergent entropic force arguments. Our study provides a clear and direct link between the local geometry of fluid structure and the properties of glass formation, independent of interaction potential or other non-geometric tuning parameters. We ultimately demonstrate that the engineering of fragility in colloidal systems via slight changes to particle shape is possible.

Graphical abstract: Particle shape tunes fragility in hard polyhedron glass-formers

Supplementary files

Article information

Article type
Paper
Submitted
08 Jun 2020
Accepted
09 Nov 2020
First published
10 Nov 2020

Soft Matter, 2021,17, 600-610

Particle shape tunes fragility in hard polyhedron glass-formers

E. G. Teich, G. van Anders and S. C. Glotzer, Soft Matter, 2021, 17, 600 DOI: 10.1039/D0SM01067G

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